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Environmental fate & pathways

Bioaccumulation: aquatic / sediment

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Endpoint:
bioaccumulation in aquatic species: fish
Type of information:
migrated information: read-across from supporting substance (structural analogue or surrogate)
Adequacy of study:
supporting study
Reliability:
2 (reliable with restrictions)
Rationale for reliability incl. deficiencies:
other: Acceptable, well documented publication which meets basic scientific principles.
Qualifier:
no guideline followed
Principles of method if other than guideline:
Brook trout (Salvelinusfontinal) about 30 d old and weighing 0.2 g were exposed for 56 d to duplicated nominal pHs of 5.0, 6.0 and 7.2 in combination with nominal aluminum concentrations of 200 μg/L. Analyses of percent mortality (arcsine transformed values), fish weight and whole-body residues of aluminum were performed.
GLP compliance:
no
Radiolabelling:
no
Details on sampling:
- Sampling intervals/frequency for test organisms:
Samples of fish were collected from each treatment for whole-body aluminium analyses on days 3, 7, 14, 28 and 56 of the exposure. During the depuration period, fish were sampled at 3, 7, 14 and 28 d for whole-body aluminum analyses. Mortality and pH were monitored daily in each treatment.

- Sample storage conditions before analysis:
The fish were cultured in a 52- x 32- x 30.5-cm (length x width x height) glass exposure aquaria equipped with 20.5 cm standpipes and held 34.1 L of exposure water. The diluter was adjusted to deliver 1 L of exposure water to each aquarium every 15 min to provide 2.8 volume replacements per day.
Details on preparation of test solutions, spiked fish food or sediment:
PREPARATION AND APPLICATION OF TEST SOLUTION (especially for difficult test substances)
- Background concentrations of aluminum in the unexposed brook trout from the laboratory culture averaged 0.68 μg/g.
- 10 μl of a 20-mg/L calcium solution to 1 ml of each water sample and standard was added before analysis as a matrix modifier to counteract the enhancing effect of calcium in the exposure water on the aluminum signal. The method of standard additions (0, 50 and 100 μg/L aluminum) for analyzing fish samples was used to correct for matrix enhancement of the aluminum signal. Samples were diluted when necessary to keep them within the linear range of the instrument (200 μg/L aluminum).
Test organisms (species):
Salvelinus fontinalis
Details on test organisms:
Eyed eggs of brook trout were obtained from Beity’s Resort, Valley, Washington. The fish were cultured in well water (alkalinity 250 mg/L and hardness 270 mg/L as CaCO3) at 17 to 18 °C until they were about 30 d old and weighed 0.2 g.
Route of exposure:
aqueous
Test type:
semi-static
Water / sediment media type:
natural water: freshwater
Total exposure / uptake duration:
56 d
Total depuration duration:
28 h
Hardness:
Alkalinity: 236-244 μeq/L
Ca content: 3.0 mg/L
Test temperature:
12 °C
pH:
5.3 - 7.2
Dissolved oxygen:
not specified
TOC:
not specified
Details on test conditions:
At the start of the test, fish were acclimated from well water (hardness of 280 mg/L as CaCO3, temperature 17 to 19 °C) to experimental water (alkalinity of 236-244 μeq/L) and test temperature (12 °C) over a 3-d period. Groups of 100 brook trout were then removed from the acclimation tanks, placed into 6 of the
12 aquaria in the proportional diluter and exposed to the pH and aluminum treatments. Appropriate amounts of an acid mixture (one-third nitric acid and two-thirds sulfuric acid v/v) and an aluminum sulfate stock solution were delivered to the diluter with automated pipettes to maintain the desired pH and aluminum treatments. After 56 d, the fish were transferred to the remaining six aquaria, in which pH alone was maintained during a 28-d depuration period. The fish were fed a Rangen@ commercial feed ad libitum twice daily during the test.
Nominal and measured concentrations:
nominal aluminum concentrations of 200 μg/L.
Reference substance (positive control):
no
Type:
BCF
Value:
215 dimensionless
Basis:
whole body w.w.
Time of plateau:
1.53 d
Calculation basis:
steady state
Remarks on result:
other: Mean exposure pH 5.3, days estimated for 90% steady state
Remarks:
Conc.in environment / dose:207 µg/L
Type:
BCF
Value:
123 dimensionless
Basis:
whole body w.w.
Time of plateau:
4.17 d
Calculation basis:
steady state
Remarks on result:
other: Mean exposure pH 6.1, days estimated for 90% steady state
Remarks:
Conc.in environment / dose:207 µg/L
Type:
BCF
Value:
36 dimensionless
Basis:
whole body w.w.
Time of plateau:
1.72 d
Calculation basis:
steady state
Remarks on result:
other: Mean exposure pH 7.2, days estimated for 90% steady state
Remarks:
Conc.in environment / dose:207 µg/L
Elimination:
yes
Parameter:
DT50
Depuration time (DT):
0.46 d
Elimination:
yes
Parameter:
DT50
Depuration time (DT):
1.26 d
Elimination:
yes
Parameter:
DT50
Depuration time (DT):
0.52 d

Results:

During the test, measured pHs were close to nominal values (see table). Measured concentrations of total aluminum were initially higher than the nominal concentrations of 200μg/L, but gradually approached the expected concentrations as the exposure

progressed (see table). Aluminum concentrations were more variable at pH 7.2 than at pH 5.3 and 6.1, probably due to differences in solubility limits.

Background concentrations of aluminum in the unexposed brook trout from the laboratory culture averaged 0.68μg/g. Aluminum concentrations in fish during the exposure period of the test ranged from 2.8 to 78μg/g, and concentrations during the

elimination period ranged from 0.7 to 5.3μg/g.

Brook trout accumulated significantly higher aluminum residues in less time at pH 5.3 than at pH 6.1 and 7.2. Tissue residues of aluminum in brook trout increased rapidly and then declined at pH 5.3 and 6.1, although exposure to aluminum was continuous. Maximum whole-body residues were reached at 3 d in the pH 5.3 treatment and 7 d at pH 6.1. Whole-body residues in brook trout

exposed to aluminum at pH 7.2 reached maximum concentrations within 3 d and then decreased gradually during the rest of the exposure period. During the depuration period, the trout from all of the treatments quickly eliminated aluminum and at 3 d

contained less than 5μg/g.

Table: Mean aluminum exposure concentration, whole-body residues (wet weight basis), weight and mortality (+ standard deviations in parentheses) for brook trout exposed at acidic and neutral pH for 56 d. Tissue residue values within pH series and concentration columns having common letters are not significantly different. Weight and mortality values within columns and time with common letters are not significantly different. Least significant difference testp0.05.

Mean pH and day of exposure

Aluminum exposure concentration (μg/L)a

Aluminum tissue concentration (μg/g)b

Weight (g)

Mortality (%)

pH 5.3 (0.5)

 

 

 

 

3

251.5 (41.7)

58.4 (7.6)a

0.25 (0.02)a

2.0 (0.0)a

7

239.0 (30.2)

46.4 (15.8)ac

0.21 (0.01)a

11.5 (3.3)a

14

214.0 (45.3)

30.3 (14.3)b

0.21 (0.01)a

21.0 (2.8)a

28

198.1 (48.5)

33.8 (5.6)bc

0.19 (0.02)a

42.5 (13.4)a

56

206.8 (9.0)

37.3 (18.0)bc

0.24 (0.07)a

73.0 (16.9)a

pH 6.1 (0.3)

 

 

 

 

3

323.5 (23.3)

18.5 (6.2)a

0.26 (0.04)a

0.0b

7

266.8 (68.9)

40.7 (19.3)b

0.21 (0.03)a

0.0b

14

223.5 (86.9)

23.2 (10.1)a

0.20 (0.03)a

3.5 (0.7)b

28

211.9 (77.8)

21.6 (10.9)a

0.20 (0.03)a

27.5 (12.0)b

56

217.1 (70.9)

16.6 (10.3)a

0.44 (0.06)a

48.0 (33.9)ab

pH 7.2 (0.1)

 

 

 

 

3

415.0 (8.5)

12.5 (1.9)a

0.27 (0.02)a

0.0b

7

305.0 (127.4)

8.3 (3.0)a

0.28 (0.03)b

0.0b

14

278.2 (108.8)

12.8 (7.1)a

0.40 (0.03)b

0.0c

28

253.6 (103.1)

9.0 (5.2)a

0.58 (0.08)b

0.0c

56

267.6 (95.7)

3.8 (0.7)a

1.50 (0.24)b

1.0 (1.4)b

a Reference water samples analyzed for quality assurance averaged 503 ± 9μg/L aluminum (established value =

460 ± 120μg/L); recovery of aluminum from spiked samples averaged 103 ± 4%; blank water samples contained

less than 5μg/L aluminum; and the limit of detection of aluminum in water was 5μg/L.

b Reference tissue samples analyzed for quality assurance averaged 19.2 ± 1.3 pg/g aluminum (established value =

21.1 ±4.6μg/g), and reference water samples averaged 489 ± 13μg/L aluminum (established value = 460 ± 120

μg/L); recovery of aluminum from spiked tissue samples averaged 102 ± 6%; blank samples contained 0.18μg/g

aluminum or less; and the limit of detection of aluminum in tissue was 0.18μg/g.

Endpoint:
bioaccumulation in aquatic species: fish
Type of information:
migrated information: read-across from supporting substance (structural analogue or surrogate)
Adequacy of study:
supporting study
Reliability:
2 (reliable with restrictions)
Rationale for reliability incl. deficiencies:
other: Acceptable, well documented publication which meets basic scientific principles.
Qualifier:
no guideline followed
Principles of method if other than guideline:
Environmental monitoring study: Smallmouth bass were collected from Chatuge Reservoir.
The total aluminum concentration in different organs (kidney, liver, gill filaments and gastroinstesines) as well as whole fish aluminum contents were investigated. The aluminum concentrations was evaluated by analysis with graphite furnace atomic absorption spectrophotometry.
GLP compliance:
no
Radiolabelling:
no
Details on sampling:
- Sample storage conditions before analysis: whole-body fish were frozen
- Test media: the background water collected from the Chatuge Reservoir (border of Georgia and North Carolina, USA). The Reservoir receives runoff from forested watersheds that are poorly buffered. And there are no known sources of significant contamination from agriculture within the watershed.
Vehicle:
no
Test organisms (species):
Micropterus dolomieui
Details on test organisms:
TEST ORGANISM
- Common name: smallmouth bass
- Source: Chatuge Reservoir
Route of exposure:
aqueous
Test type:
field study
Water / sediment media type:
natural sediment: freshwater
Hardness:
Mean alkalinity: 140 µequiv/L
pH:
average: 6.3 for 52 measurements over a 6-year period.
Details on test conditions:
All dissection tools and homogenization equipments were rinsed withdiluted HCl and then ultrapure water (15-18 MΩ-cm specific resistivity) before each sample was processed. Forzen fish used for whole-body analysis were sectioned with a band saw and passed twice through a small meat grinder. Fish which were dissected before analysis were placed on a clean polyethlyene sheet, and the liver, kidney, gill filaments, and gastrointestinal tract were removed with stainless steel scalpels and surgical scissors. The gastrointestinal tract was sliced open, and the contents were flushed into pre-leached beakers with ultrapure water. Large, intact food items were removed and not included in the analysis of the gut contents. Analysis of gut tissue included the stomach, intestine, and pyloric caeca. The remaining carcass was homogenized by chopping it into sections on a Teflon cutting board and then passing it 3 times through a small meat grinder.
Nominal and measured concentrations:
Measured natural concentrations ranged from 0.06 to 0.94 mg/L total Al within the not further specified study period.
Reference substance (positive control):
no

Results:

Inclusion of gastrointestinal tract contents contained highly variable amounts of aluminium and caused bias and increased variability when included in whole-body fish. Since aluminium concentrations in tissues of stomach and intestine were similar to those in the whole body (less gastrointestinal tract contents), the entire gastrointestinal tract and contents could be removed to reduce bias and variability without measurably altering the true whole-body aluminium concentrations. Of the organs analyzed, gill filaments had the highest and most variable aluminium concentrations and may have contributed to within-fish whole-body variability because of incomplete homogenization.

 

Aluminium Concentrations (μg/g Wet Weight) in Selected Tissues of Smallmouth Bass

(the aluminium concentration in background water is 0.06-0.94 mg/L)

carcassa

gill

liver

kidney

gut

Whole bodyb(less gut content)

Whole bodyb(with gut content)

Range ( results from 10 tests)

1.1 – 10.2

3.8 - 198

0.5 – 4.6

< 1.0 – 2.0

1.3 – 31.5c

1.2 – 12.3

1.3 – 97.4

Mean ± SD

3.0 ± 2.8

58 ± 64

1.5 ± 1.2

< 1.0

2.5 ± 1.1

3.9 ± 3.6

13.8 ± 29.5

a values are means of two determinations.

b Estimated by summing all parts according to percent body weight.

c Not included in determination of mean and SD.

Endpoint:
bioaccumulation in aquatic species: fish
Type of information:
migrated information: read-across from supporting substance (structural analogue or surrogate)
Adequacy of study:
supporting study
Reliability:
2 (reliable with restrictions)
Rationale for reliability incl. deficiencies:
other: Acceptable, well documented publication which meets basic scientific principles.
Qualifier:
no guideline followed
Principles of method if other than guideline:
Field study: Trout were collected from Medical Lake (Spokane County, Washington, USA), an aluminum sulphate treated water body (to control eutrophication). Liver, kidney, stomach, muscle, gill, heart and reproductive tissues were then tested for total aluminum content (atomic absorption spectrophotometry).
GLP compliance:
no
Radiolabelling:
no
Details on sampling:
- Sampling intervals/frequency for test organisms:
Rainbow trout from Medical Lake were caught using trammel and gill nets (Sept-Nov 1979 and Mar-Oct 1980). Trout were also obtained from the North Spokane Griffith's Spring Hatchery in September 1980. Additional trout from untreated regional lakes (West Medical, Badger and North Silver lakes) were collected in August and September 1980.
- Sampling intervals/frequency for test medium samples:
Medical Lake plankton and water samples were usually collected monthly from June 1979 through October 1980. A bottom-to-surface oblique tow was made with a 76 micron silk net to obtain plankton samples.
- Sample storage conditions before analysis:
Trout were weighed, measured, tagged and frozen. Liver, kidney, stomach, muscle, gill, heart and reproductive tissues were excised from defrosted fish and wet weights redetermined. A composite sample of the water column was acidified (pH < 2) and frozen in acid-washed bottles to await further analysis. The plankton samples were filtered (0.45 microns) and frozen in acid-washed vials.
- Details on sampling and analysis of test organisms and test media samples (e.g. sample preparation, analytical methods):
Due to the small size of the 0+ fish obtained from the hatchery and from the untreated lakes, composite tissue samples were taken. Tissues dissected from Medical lake fish collected in July 1980 were used to determine wet weight to dry relationships. Both fish tissue and plankton wet weight to dry weight conversion factors were determined afer drying the samples at 105 °C for 24 hours.
Vehicle:
no
Test organisms (species):
Oncorhynchus mykiss (previous name: Salmo gairdneri)
Route of exposure:
aqueous
Test type:
field study
Water / sediment media type:
natural sediment: freshwater
Hardness:
Medical Lake exhibits relatively high alkalinity (approximately 12 me/L HCO3-) with a pH near 9.
pH:
around 9
Nominal and measured concentrations:
Jun 1979-Oct 1980: Total aluminum concentrations ranged between 0.16 and 0.75 mg/L; dissolved aluminum ranged between 0.09 and 0.42 mg/L.
Water from North Silver and West Medical lakes contained total and dissolved aluminium levels less than 0.0001 mg/L.

Results:

Differential accumulation of aluminium in the tissues occurred in all age classes oftrout. There was a greater than six-fold increase in aluminium levels for liver and kidney with increasing age (0+ to 2+). The overall changes in aluminium content with increasing age for stomach, muscle, and heart were not as marked. Gill tissue, although not showing marked changes with age, was substantially elevated in aluminium. Analysis of reproductive tissue revealed a 20-fold increase in aluminium between 1+ and 2+ fish.

Table below: Total aluminum concentrations (mg/g tissue or organ dry weight) in selected trout (Oncorhynchus mykiss) tissues.

 

Age group 

Tissue

0 yrs +

1 yrs +

2 yrs +

Liver

0.59 ± 1.66

1.41 ± 1.20

3.99 ± 1.50

Kidney

0.39± 0.81

1.03± 1.54

2.51± 1.27

Stomach

0.70± 1.78

0.70± 0.89

0.67± 0.83

Muscle

0.18± 0.70

0.05± 0.18

0.14± 0.50

Gill

6.25± 4.54

5.88± 3.58

3.08± 3.45

Heart

0.19± 0.39

0.28± 0.66

0.38± 1.06

Reproductive

**

0.07± 0.12

1.50± 1.37

Total aluminium levels in tissues taken from 0+ and 1+ fish of untreated lakes indicated a decline in concentrations in both liver and kidney. There was little change in aluminium content for stomach, but muscle increased more than three-fold. Gill tissue displayed elevated aluminium levels, whereas in heart tissue there was a 34-fold decline with increasing age.

Aluminium levels in the plankton were approximately ten time greater (dry weight comparison) than any encountered the trout tissues. Plankton may absorb the aluminate ion on the body surface. There may also be ingestion of particulate aluminium complexes by filter-feeding zooplankton.

Statistical comparisons of experimental and control tissues revealed few overall significant differences (P = 0.05) in the level of aluminium between alum-exposed and non-exposed fish, but significant differences existed between tissues within a given treatment and age class.

Endpoint:
bioaccumulation in aquatic species: fish
Data waiving:
other justification
Justification for data waiving:
other:

Description of key information

Key value for chemical safety assessment

Additional information

In general, metals do not biomagnify unless they are present as, or having the potential to be, in an organic form (e. g. methylmercury). Organometals tend to be lipid soluble, are not metabolized, and are efficiently assimilated upon diet borne exposure. The available evidence shows the absence of aluminium biomagnification across trophic levels both in the aquatic and terrestrial food chains. The existing information suggests not only that aluminium does not biomagnify, but rather that it tends to exhibit biodilution at higher trophic levels in the food chain. More detailed information can be found in the attached document (White paper on waiving for secondary poisoning for Al & Fe compounds final report, March, 2010. pdf). BCFs for Aluminium can be found to range from quite low (~100) to quite high values (11,000) – see attached pdf on White paper for waiving secondary poisoning for iron and Aluminium. This variance can in large part be explained by the difference in exposure conditions for the various studies. The inverse relationship between water and BCF/BAF values limits the ability to describe hazard as a result of the size of the BCF, i. e., the most pristine ecosystems have the highest BCFs. A better approach is to directly assess the concentrations of Al at various trophic levels in the ecosystem.

 

Herrmann and Frick (1995) studied the accumulation of aluminium at low pH conditions in benthic invertebrates with time and representing different functional feeding groups (predators and detritus feeders). Invertebrates of different taxa and feeding type were collected in springtime, when acidity and Al levels mostly increase from seven streams in southern. Four of the streams typically had pH values of 4 - 4.5 and contained 0.40 - 0.70 mg inorganic Al/L. The other three streams showed pH values around 6 and Al concentrations of 0.05 mg inorganic Al/l. For most taxa that could be compared, the animals from the most acidic streams (pH 4) contained more Al than those from the less acid streams (pH 6). At both pH levels there was a clear tendency that predators contained significantly less amounts of aluminium than shredders. The latter results do not support the hypothesis that aluminium can be accumulated along a food chain in an acidic environment.

 

When diluted in the aquatic environment, the registered substance reaction mass of aluminate sulfate and aluminium nitrate is hydrolysed rapidly to form insoluble aluminium hydroxide and free sulfate and nitrate. The introduced nitrate can be degraded by many microorganisms to gaseous nitrogen, which is environment-friendly and degases from the water circuit.

Bioconcentration of aluminium in fish is a function of the water quality (e.g. pH and total organic carbon). Cleveland et al. (1991) maintained brook trout (Salvelinus fontinal) in water containing 200 µg/L total aluminium at pH values of 5.0, 6.0 and 7.2 for 56 days. Estimated steady state bioconcentration factors (BCFs) for aluminium were 215 at pH 5.3, 123 at pH 6.1 and 36 at pH 7.2, respectively. The estimated time to reach a 90% steady state was 1.5 days at pH 5.3, 4.2 days at pH 6.1 and 1.7 days at pH 7.2. These data demonstrate that the BCFs are inversely related to pH. Elimination during the 28-day depuration phase was more rapid at pH 5.3 than at pH 6.1 or 7.2. The biological half-life of aluminium in brook trout was 0.46 day at pH 5.3, 1.26 day at pH 6.1 and 0.52 day at pH 7.2. The distribution of aluminium accumulation in smallmouth bass (Micropterus dolomieui) investigated by Brumbaugh and Kane (1985) showed that aluminium concentration in tissues of stomach and intestine were similar to those in the whole body. Of the organs analysed, gill filaments had the highest and most variable aluminium concentration. Berg et al. (1985) determined aluminium concentrations in organs under field conditions. In rainbow trout (Oncorhynchus mykiss) at the age of one year, aluminium has been found predominantly in gills. In two years old fish, the aluminium concentration in liver was similar to that in gill the patterns of aluminium accumulation in fish by these studies may explain the elimination mechanisms of aluminium. Additionally, aluminium has been shown (Jagoe et al. 1987) to cause a progression of severe gill damage in Atlantic salmon (Salmo salar) at low pH. If the gills of fish were damaged during the studies, the capacity of the fish to take up aluminium may have been progressively impaired during the exposure and resulted in decreased survival and growth and a relative lower critical body burden in fish.

 

Steady state BCF values as high as 14,000 have been reported in Asellus aquaticus after a 20 day exposure to aluminium (Goossenaerts and Grieken, 1988). Similar, a steady state BCF of 19, 000 was reported for the gut tissue of the freshwater snail Lymnaea stagnalis by Elangovan et al., (1997). Moreover, high aluminium concentrations were determined in plankton (Buergel, 1983). However, much of the accumulation was due to passive adsorption of aluminium onto the cuticle. Therefore, these BCFs are not representative of the internal concentration of aluminium and overestimate accumulation in these species.

 

Based on the data available, aluminium is considered to have a low bioaccumulation potential to aquatic organisms under circum neutral conditions. In the acidic aquatic environment, aluminium demonstrates a moderate bioaccumulation potential. The high BCFs observed in aquatic invertebrates and high concentration found in planktons is not representative of the internal concentration of aluminium and overestimate accumulation in these species.

 

Reference

Jagoe, C.H., et al.(1987) Abnormal gill development in Atlantic salmon (Salmo solar) fry exposed to aluminium at low pH, Ann Soc R Zoo1 Belg 117 375-386

 

Goossenaerts C. and Grieken R. V. (1988) A microanalytical study of the gills of aluminium exposed rainbow trout (Oncorhynchus mykiss). International Journal of Environmental Analysis and Chemistry, 34, 227–237.

 

Elangovan R, et al.(1997) Bioaccumulation of aluminium in the freshwater snail Lymnaea stagnalis at neutral pH. Environmental Pollution,96, No. 1, 29–33.

 

Environmenta Agnecy (2007) Proposed EQS for Water Framework Directive Annex VIII, Substances: aluminium (inorganic monometric), Science Report: SC040038/SR1; SNIFER Report: WFD52 (i); ISBN: 978 -1 -84432 -651 -8, Feb 2007